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    Field-Free Three Dimensional Molecular Axis Alignment

    Jonathan G. Underwood1,*, Benjamin J. Sussman2,3, and Albert Stolow2,3

    • 1Department of Physics and Astronomy, The Open University, Walton Hall, Milton Keynes, United Kingdom, MK7 6AA
    • 2Steacie Institute for Molecular Sciences, National Research Council of Canada, 100 Sussex Drive, Ottawa, Ontario, K1A 0R6, Canada
    • 3Department of Physics, Queen’s University, Kingston, Ontario, K7L 3N6, Canada
    • *Electronic address: j.underwood@open.ac.uk

    Phys. Rev. Lett. 94, 143002 – Published 13 April, 2005

    DOI: https://doi.org/10.1103/PhysRevLett.94.143002

    Abstract

    We investigate strategies for field-free three dimensional molecular axis alignment using strong nonresonant laser fields under experimentally realistic conditions. Using the polarizabilites and rotational constants of an asymmetric top rotor molecule (ethene, C2H4), we consider three different methods for axis alignment of a Boltzmann distribution of rotors at 4 K. Specifically, we compare the use of impulsive kick laser pulses having both linear and elliptical polarization to the use of elliptically polarized switched laser pulses. We show that an enhanced degree of field-free three dimensional alignment of ground vibronic state molecules obtains from the use of two orthogonally polarized, time-separated laser pulses.

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